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1.
J Environ Sci (China) ; 148: 274-282, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39095164

RESUMO

Developing cost-effective and high-performance catalyst systems for dry reforming of methane (DRM) is crucial for producing hydrogen (H2) sustainably. Herein, we investigate using iron (Fe) as a promoter and major alumina support in Ni-based catalysts to improve their DRM performance. The addition of iron as a promotor was found to add reducible iron species along with reducible NiO species, enhance the basicity and induce the deposition of oxidizable carbon. By incorporating 1 wt.% Fe into a 5Ni/10ZrAl catalyst, a higher CO2 interaction and formation of reducible "NiO-species having strong interaction with support" was observed, which led to an ∼80% H2 yield in 420 min of Time on Stream (TOS). Further increasing the Fe content to 2wt% led to the formation of additional reducible iron oxide species and a noticeable rise in H2 yield up to 84%. Despite the severe weight loss on Fe-promoted catalysts, high H2 yield was maintained due to the proper balance between the rate of CH4 decomposition and the rate of carbon deposit diffusion. Finally, incorporating 3 wt.% Fe into the 5Ni/10ZrAl catalyst resulted in the highest CO2 interaction, wide presence of reducible NiO-species, minimum graphitic deposit and an 87% H2 yield. Our findings suggest that iron-promoted zirconia-alumina-supported Ni catalysts can be a cheap and excellent catalytic system for H2 production via DRM.


Assuntos
Óxido de Alumínio , Hidrogênio , Ferro , Metano , Níquel , Zircônio , Metano/química , Zircônio/química , Catálise , Ferro/química , Hidrogênio/química , Óxido de Alumínio/química , Níquel/química
2.
Int J Biol Macromol ; 278(Pt 3): 134935, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39179088

RESUMO

For the first time, Frankincense resin (FR) has been carboxymethylated to produce CMFR - AuNPs and the conjugate was utilized for the Doxorubicin drug loading. The carboxymethylation of the carboxylic, phenolic, and hydroxyl functional groups of FR has been developed into carboxymethylated Frankincense resin (CMFR). A novel CMFR-AuNPs was synthesized using the developed CMFR as a stabilizing and reducing agent. The antibacterial, antioxidant, and in-vitro anticancer activities were investigated by using CMFR-AuNPs and CMFR - AuNPs@DOX. CMFR-AuNPs demonstrated antioxidative properties by quenching DPPH radicals effectively. CMFR-AuNPs and DOX@CMFR-AuNPs demonstrated strong antibacterial activity against K. pneumoniae, S. aureus, B. subtilis, and E. coli. The cell viability was tested for CMFR -AuNPs at various concentrations of Dox-loaded CMFR -AuNPs (CMFR-AuNPs + Dox1, CMFR-AuNPs + Dox 2, & CMFR-AuNPs + Dox 3). The highest inhibition was observed on MCF-7 and HeLa cell lines using CMFR-AuNPs + Dox 3, respectively. Various techniques such as UV, FTIR, TGA, XRD, SEM, EDAX and TEM were used to characterize the designed CMFR and CMFR-AuNPs. After carboxy methylation, the amorphous nature of FR changed to crystallinity, as reflected in the XRD spectra. The XRD spectrum of the CMFR- AuNPs showed FCC structure due to the involvement of hydroxyl and carboxylic functional groups of CMFR strongly bound with the AuNPs. TGA results revealed that the CMFR is thermally more stable than FR. TEM revealed that CMFR - AuNPs were well dispersed, spherical, and hexagonal with an average diameter of 7 to 10 nm, while the size of doxorubicin loaded (DOX@CMFR-AuNPs) AuNPs was 11 to 13 nm. Green CMFR-AuNPs have the potential to enhance the drug loading and anticancer efficacy of drugs.


Assuntos
Antineoplásicos , Antioxidantes , Doxorrubicina , Ouro , Nanopartículas Metálicas , Ouro/química , Nanopartículas Metálicas/química , Humanos , Antioxidantes/farmacologia , Antioxidantes/química , Antineoplásicos/farmacologia , Antineoplásicos/química , Doxorrubicina/química , Doxorrubicina/farmacologia , Resinas Vegetais/química , Antibacterianos/farmacologia , Antibacterianos/química , Células MCF-7 , Células HeLa , Sobrevivência Celular/efeitos dos fármacos , Sinergismo Farmacológico
3.
Nanomaterials (Basel) ; 14(15)2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-39120425

RESUMO

Global warming, driven by greenhouse gases like CH4 and CO2, necessitates efficient catalytic conversion to syngas. Herein, Ni containing different molecular sieve nanomaterials are investigated for dry reforming of methane (DRM). The reduced catalysts are characterized by surface area porosity, X-ray diffraction, Raman infrared spectroscopy, CO2 temperature-programmed desorption techniques, and transmission electron microscopy. The active sites over each molecular sieve remain stable under oxidizing gas CO2 during DRM. The reduced 5Ni/CBV10A catalyst, characterized by the lowest silica-alumina ratio, smallest surface area and pore volume, and narrow 8-ring connecting channels, generated the maximum number of active sites on its outer surface. In contrast, the reduced-5Ni/CBV3024E catalyst, with the highest silica-alumina ratio, more than double the surface area and pore volume, 12-ring sinusoidal porous channels, and smallest Ni crystallite, produced the highest H2 output (44%) after 300 min of operation at 700 °C, with a CH4:CO2 = 1:1, P = 1 atom, gas hour space velocity (GHSV) = 42 L gcat-1 h-1. This performance was achieved despite having 25% fewer initial active sites, suggesting that a larger fraction of these sites is stabilized within the pore channels, leading to sustained catalytic activity. Using central composite design and response surface methodology, we successfully optimized the process conditions for the 5Ni/CBV3024E catalyst. The optimized conditions yielded a desirable H2 to CO ratio of 1.00, with a H2 yield of 91.92% and a CO yield of 89.16%, indicating high efficiency in gas production. The experimental results closely aligned with the predicted values, demonstrating the effectiveness of the optimization approach.

4.
RSC Adv ; 14(35): 25273-25288, 2024 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-39139230

RESUMO

Achieving remarkable H2 yield with significantly high H2/CO over Ni-based catalysts through partial oxidation of methane (POM) is a realistic approach to depleting the concentration of CH4 and using H2 and CO as synthetic feedstock. This study examined Ni catalysts on titania-zirconia for methane conversion via POM at 600 °C and atmospheric pressure. The addition of strontium to the catalyst was explored to improve its performance. Catalysts were characterized by X-ray diffraction, Raman-infrared-UV-vis spectroscopy, and Temperature-programmed reduction-desorption techniques (TPR, TPD). 2.5 wt% Sr addition induced the formation of the highest concentration of extreme basic sites. Interestingly, over the unpromoted catalyst, active sites are majorly generated by hardly reducible NiO species whereas upon 2.5 wt% promoted Sr promotional addition, most of active sites are derived by easily reducible NiO species. 45% CH4 conversion and 47% H2 yield with H2/CO = 3.5 were achieved over 2.5 wt% Sr promoted 5Ni/30TiO2 + ZrO2 catalyst. These results provide insight into the role of basic sites in enhancing activity through switching indirect pathways over direct pathways for POM. Further process optimization was carried out in the range of 10 000-22 000 SV, 0.35-0.75 O2/CH4, and 600-800 °C reaction temperature over 5Ni2.5Sr/30TiO2 + ZrO2 by using central composite design under response surface methodology. The optimum activity as high as ∼88% CH4 conversion, 86-87% yield of H2, and 2.92H2/CO were predicted and experimentally validated at 800 °C reaction temperature, 0.35O2/CH4 ratio, and 10 000 space velocity.

5.
ACS Omega ; 9(24): 25800-25811, 2024 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-38911787

RESUMO

The copper/nickel-metal on commercial H-Beta zeolite supports was synthesized with different wt % (Ni) of 5, 10, 15, and 20, and was used in the cyclohexene epoxidation process. The synthesized catalyst has been used in a continuous reactor for the cyclohexene epoxidation process, with mild conditions and H2O2 as an oxidant. The catalytic performance was ascertained by adjusting parameters such as the temperature, pressure, WHSV, reaction time, and solvents. The catalytic performance showed the resulting yield in both cyclohexene conversion and selectivity was more than 98.5%. The catalyst's textural attributes, morphology, chemical composition, and stability were determined using FT-IR, XRD, BET, HR-SEM, and TPD. The most active catalyst among those that were synthesized was evaluated, and the reaction parameters were selected to optimize yield and conversion. The H-Beta/Cu/Ni (15%) catalyst has the best conversion (98.5%) and selectivity (100%) for cyclohexene among the catalysts examined. Cu and Ni(15%) metals were successfully added to the H-Beta zeolite, causing little damage to the crystalline structure and resulting in good reusability over five cycles, as well as little loss of catalytic selectivity. Acetonitrile was the solvent that provided the highest conversion and selectivity among the others. These findings show that H-Beta/Cu/Ni bimetallic catalysts have the potential to be effective epoxidation catalysts. Because of their outstanding conversion and selectivity, the continuous reaction technique used in this work makes them appropriate for industrial production-level applications.

6.
ACS Omega ; 9(18): 20322-20330, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38737024

RESUMO

This study addresses the pivotal challenge of hydrogen production through methane decomposition, offering a pathway to achieving clean energy goals. Investigating the utilization of titania-modified zirconia dual redox supports (10TiZr) in iron or doped iron-based catalysts for the CH4 decomposition reaction, our research involves a thorough characterization process. This includes analyses of the surface area porosity, X-ray diffraction, Raman-infrared spectroscopy, and temperature-programmed reduction/oxidation. The observed sustained enhancement in catalytic activity over extended durations suggests the in situ formation of catalytically active sites. The introduction of Co or Ni into the 30Fe/10TiZr catalyst leads to the generation of a higher density of reducible species. Furthermore, the Ni-promoted 30Fe/10TiZr catalyst exhibits a lower crystallinity, indicating superior dispersion. Notably, the cobalt-promoted 30Fe/10TiZr catalyst achieves over 80% CH4 conversion and H2 yield within 3 h. Additionally, the Ni-promoted 30Fe/10TiZr catalyst attains a remarkable 87% CH4 conversion and 82% H2 yield after 3 h of the continuous process.

7.
Nanomaterials (Basel) ; 14(8)2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38668225

RESUMO

Drinking water defluoridation has attracted significant attention in the scientific community, from which membrane technology, by exploring thin film nanocomposite (TFN) membranes, has demonstrated a great potential for treating fluoride-contaminated water. This study investigates the development of a TFN membrane by integrating titanium oxide nanosheets (TiO2 NSs) into the polyamide (PA) layer using interfacial polymerization. The characterization results suggest that successfully incorporating TiO2 NSs into the PA layer of the TFN membrane led to a surface with a high negative charge, hydrophilic properties, and a smooth surface at the nanoscale. The TFN membrane, containing 80 ppm of TiO2 NSs, demonstrated a notably high fluoride rejection rate of 98%. The Donnan-steric-pore-model-dielectric-exclusion model was employed to analyze the effect of embedding TiO2 NSs into the PA layer of TFN on membrane properties, including charge density (Xd), the pore radius (rp), and pore dielectric constant (εp). The results indicated that embedding TiO2 NSs increased Xd and decreased the εp by less than the TFC membrane without significantly affecting the rp. The resulting TFN membrane demonstrates promising potential for application in water treatment systems, providing an effective and sustainable solution for fluoride remediation in drinking water.

8.
ACS Omega ; 9(8): 9309-9320, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38434824

RESUMO

Zirconia-alumina-supported Ni (5Ni/10ZrO2+Al2O3) and Sr-promoted 5Ni/10ZrO2+Al2O3 are prepared, tested for carbon dioxide (CO2) methanation at 400 °C, and characterized by X-ray diffraction, X-ray photoelectron spectroscopy, surface area and porosity, infrared spectroscopy, and temperature-programmed reduction/desorption techniques. The CO2 methanation is found to depend on the dispersion of Nickel (Ni) sites as well as the extent of stabilization of CO2-interacted species. The Ni active sites are mainly derived from the reduction of 'moderately interacted NiO species'. The dispersion of Ni over 1 wt % Sr-promoted 5Ni/10ZrO2+Al2O3 is 1.38 times that of the unpromoted catalyst, and it attains 72.5% CO2 conversion (against 65% over the unpromoted catalyst). However, increasing strontium (Sr) loading to 2 wt % does not affect the Ni dispersion much, but the concentration of strong basic sites is increased, which achieves 80.6% CO2 conversion. The 5Ni4Sr/10ZrO2+Al2O3 catalyst has the highest density of strong basic sites and the highest concentration of active sites with maximum Ni dispersion. This catalyst displays exceptional performance and achieves approximately 80% CO2 conversion and 70% methane (CH4) yield for up to 25 h on steam. The unique acidic-basic profiles composed of strong basic and moderate acid sites facilitate the sequential hydrogenation of formate species in the COx-free CH4 route.

9.
RSC Adv ; 14(11): 7728-7739, 2024 Feb 29.
Artigo em Inglês | MEDLINE | ID: mdl-38444966

RESUMO

This work examines the hydrodeoxygenation (HDO) activity of non-edible oils using a high surface area catalyst. The HDO activity was thoroughly examined and contrasted using the high surface area catalyst Ni/Pt-ZSM-5 as well as other supports like MCM-48 and H-beta. Ni/Pt bimetals supported on mesoporous ZSM-5 were created via reverse order impregnation to facilitate HDO of non-edible oils. Techniques such as XRD, FT-IR, BET, HR-TEM, HR-SEM, TPD, and TGA were used to characterize the produced catalysts. The synthesized catalysts considerably influenced the hydrodeoxygenation activities for the synthesis of lengthy chain hydrocarbons in a stainless-steel reactor with a high-pressure fixed bed between 300 and 375 °C under 10-40 bar hydrogen pressure. High levels of Ni/Pt-ZSM-5 acidity, textural, and H2 consumption qualities were discovered. Distributions of the products were also reviewed, along with comparisons of the structure-activity connections.

10.
RSC Adv ; 14(4): 2300-2310, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38213975

RESUMO

A wetness impregnation method was used to impregnate the substrate with a substantial quantity of oleic acid together with a metal precursor, leading to significantly dispersed Ni-Fe bimetallic catalysts based on mesoporous SBA-15. Using a wide variety of characterization methods, such as XRD, BET, and TEM Analysis, the physiochemical properties of the catalyst were determined. The addition of the metal does not have any effect on the structural characteristics of the SBA-15 catalyst, as validated by transmission electron microscopy (TEM), which shows that the prepared SBA-15 supported catalyst has a hexagonal mesoporous structure. The catalytic capabilities of the Ni-Fe-SBA-15 catalysts were evaluated in the conversion of BzOH using tert-butyl hydroperoxide (TBHP) as an oxidant and acetonitrile as a solvent. The Ni/Fe-SBA-15 (NFS-15) catalytic composition is the best of the developed catalysts, with a maximum conversion of 98% and a selectivity of 99%. In-depth investigations were conducted into the molar ratio of TBHP to BzOH, the dosage of the catalyst, the reaction rate, temperature, and solvent. The recycling investigations indicate that the synthesized Ni/Fe-SBA-15 (NFS-15) catalyst seems to be more durable up to seven successive cycles.

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